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Green Electrosynthesis of 5,5′-Azotetrazolate Energetic Materials Plus Energy-Efficient Hydrogen Production Using Ruthenium Single-Atom Catalysts
Advanced Materials ( IF 29.4 ) Pub Date : 2022-06-20 , DOI: 10.1002/adma.202203900
Jiachen Li 1, 2 , Cong Zhang 1 , Chi Zhang 1 , Huijun Ma 3 , Zhaoqi Guo 1 , Chenglin Zhong 4 , Ming Xu 5 , Xuanjun Wang 6 , Yaoyu Wang 2 , Haixia Ma 1 , Jieshan Qiu 7
Affiliation  

Water electrolysis involves two parallel reactions, that is, oxygen evolution (OER) and hydrogen evolution (HER), in which sluggish OER is a significant limiting step that results in high energy consumption. Coupling the thermodynamically favorable electrooxidation of organic alternatives to value-added fine chemicals HER is a promising approach for the simultaneous cost-effective production of value-added chemicals and hydrogen. Here, a new coupling system for the green electrochemical synthesis of organic energetic materials (EMs) plus hydrogen production using single-atom catalysts is introduced. The catalysts are prepared by the facile galvanostatic deposition of ruthenium single atoms on the molybdenum selenide and reveal a low HER overpotential of 38.9 mV at −10 mA cm−2 in an alkaline medium. Importantly, the cell voltage of water electrolysis can be significantly reduced to only 1.35 V at a current of 10 mA cm−2 by coupling water splitting with the electrooxidation of 5-amino-1H-tetrazole to synthesize 5,5′-azotetrazolate energetic material. These materials are traditionally synthesized under harsh conditions involving a strong oxidizing agent, high-temperature conditions, and difficult separation of by-products. This study provides a green and efficient method of synthesizing organic EMs while simultaneously producing hydrogen.

中文翻译:

5,5'-偶氮四唑高能材料的绿色电合成以及使用钌单原子催化剂的节能制氢

水电解涉及两个平行反应,即析氧(OER)和析氢(HER),其中缓慢的OER是导致高能耗的重要限制步骤。将有机替代品的热力学上有利的电氧化与增值精细化学品 HER 相结合是一种有前途的方法,可以同时经济高效地生产增值化学品和氢气。在这里,介绍了一种用于绿色电化学合成有机含能材料 (EM) 以及使用单原子催化剂制氢的新耦合系统。该催化剂通过钌单原子在硒化钼上的简单恒电流沉积制备,在-10 mA cm -2下显示出38.9 mV的低HER过电位在碱性介质中。重要的是,通过将水分解与5-氨基-1 H-四唑的电氧化结合以合成高能5,5'-偶氮四唑盐,在10 mA cm -2的电流下,水电解的电池电压可以显着降低至仅1.35 V材料。这些材料传统上是在苛刻的条件下合成的,包括强氧化剂、高温条件和难以分离的副产物。本研究提供了一种绿色高效的合成有机 EMs 同时生产氢气的方法。
更新日期:2022-06-20
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